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FR2471977A1 - PROCESS FOR THE PREPARATION OF OXIME OF 3- (4-PYRIDINYL) -2-CYCLOHEXENE-1-ONE - Google Patents

PROCESS FOR THE PREPARATION OF OXIME OF 3- (4-PYRIDINYL) -2-CYCLOHEXENE-1-ONE Download PDF

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FR2471977A1
FR2471977A1 FR8021518A FR8021518A FR2471977A1 FR 2471977 A1 FR2471977 A1 FR 2471977A1 FR 8021518 A FR8021518 A FR 8021518A FR 8021518 A FR8021518 A FR 8021518A FR 2471977 A1 FR2471977 A1 FR 2471977A1
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pyridinyl
oxime
cyclohexen
oxo
mixture
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Rudolf Oesterlin
Peter Arthur Pareene
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STWB Inc
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Sterling Drug Inc
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D213/00Heterocyclic compounds containing six-membered rings, not condensed with other rings, with one nitrogen atom as the only ring hetero atom and three or more double bonds between ring members or between ring members and non-ring members
    • C07D213/02Heterocyclic compounds containing six-membered rings, not condensed with other rings, with one nitrogen atom as the only ring hetero atom and three or more double bonds between ring members or between ring members and non-ring members having three double bonds between ring members or between ring members and non-ring members
    • C07D213/04Heterocyclic compounds containing six-membered rings, not condensed with other rings, with one nitrogen atom as the only ring hetero atom and three or more double bonds between ring members or between ring members and non-ring members having three double bonds between ring members or between ring members and non-ring members having no bond between the ring nitrogen atom and a non-ring member or having only hydrogen or carbon atoms directly attached to the ring nitrogen atom
    • C07D213/24Heterocyclic compounds containing six-membered rings, not condensed with other rings, with one nitrogen atom as the only ring hetero atom and three or more double bonds between ring members or between ring members and non-ring members having three double bonds between ring members or between ring members and non-ring members having no bond between the ring nitrogen atom and a non-ring member or having only hydrogen or carbon atoms directly attached to the ring nitrogen atom with substituted hydrocarbon radicals attached to ring carbon atoms
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D213/00Heterocyclic compounds containing six-membered rings, not condensed with other rings, with one nitrogen atom as the only ring hetero atom and three or more double bonds between ring members or between ring members and non-ring members
    • C07D213/02Heterocyclic compounds containing six-membered rings, not condensed with other rings, with one nitrogen atom as the only ring hetero atom and three or more double bonds between ring members or between ring members and non-ring members having three double bonds between ring members or between ring members and non-ring members
    • C07D213/04Heterocyclic compounds containing six-membered rings, not condensed with other rings, with one nitrogen atom as the only ring hetero atom and three or more double bonds between ring members or between ring members and non-ring members having three double bonds between ring members or between ring members and non-ring members having no bond between the ring nitrogen atom and a non-ring member or having only hydrogen or carbon atoms directly attached to the ring nitrogen atom
    • C07D213/24Heterocyclic compounds containing six-membered rings, not condensed with other rings, with one nitrogen atom as the only ring hetero atom and three or more double bonds between ring members or between ring members and non-ring members having three double bonds between ring members or between ring members and non-ring members having no bond between the ring nitrogen atom and a non-ring member or having only hydrogen or carbon atoms directly attached to the ring nitrogen atom with substituted hydrocarbon radicals attached to ring carbon atoms
    • C07D213/44Radicals substituted by doubly-bound oxygen, sulfur, or nitrogen atoms, or by two such atoms singly-bound to the same carbon atom
    • C07D213/53Nitrogen atoms
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D213/00Heterocyclic compounds containing six-membered rings, not condensed with other rings, with one nitrogen atom as the only ring hetero atom and three or more double bonds between ring members or between ring members and non-ring members
    • C07D213/02Heterocyclic compounds containing six-membered rings, not condensed with other rings, with one nitrogen atom as the only ring hetero atom and three or more double bonds between ring members or between ring members and non-ring members having three double bonds between ring members or between ring members and non-ring members
    • C07D213/04Heterocyclic compounds containing six-membered rings, not condensed with other rings, with one nitrogen atom as the only ring hetero atom and three or more double bonds between ring members or between ring members and non-ring members having three double bonds between ring members or between ring members and non-ring members having no bond between the ring nitrogen atom and a non-ring member or having only hydrogen or carbon atoms directly attached to the ring nitrogen atom
    • C07D213/24Heterocyclic compounds containing six-membered rings, not condensed with other rings, with one nitrogen atom as the only ring hetero atom and three or more double bonds between ring members or between ring members and non-ring members having three double bonds between ring members or between ring members and non-ring members having no bond between the ring nitrogen atom and a non-ring member or having only hydrogen or carbon atoms directly attached to the ring nitrogen atom with substituted hydrocarbon radicals attached to ring carbon atoms
    • C07D213/44Radicals substituted by doubly-bound oxygen, sulfur, or nitrogen atoms, or by two such atoms singly-bound to the same carbon atom
    • C07D213/46Oxygen atoms
    • C07D213/50Ketonic radicals

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Pyridine Compounds (AREA)

Abstract

L'INVENTION CONCERNE UN PROCEDE AMELIORE DE PREPARATION DE L'OXIME DE LA 3-(4-PYRIDINYL)-2-CYCLOHEXENE-1-ONE A PARTIR DU 5-OXO-2-(4-PYRIDINYL) CARBONYL HEXANOATE D'ETHYLE DANS UNE SERIE DE REACTIONS EN UN SEUL RECIPIENT, QUI CONSISTE D'ABORD A CHAUFFER LE 5-OXO-2-(4-PYRIDINYL)-CARBONYLHEXANOATE D'ETHYLE AVEC UN EXCES D'ACIDE SULFURIQUE, A NEUTRALISER L'EXCES D'ACIDE, A EXTRAIRE LA 3-(4-PYRIDINYL)-2-CYCLOHEXENE-1-ONE RESULTANTE AVEC DE L'ALCOOL ISOPROPYLIQUE, A ENLEVER LA COUCHE AQUEUSE PLUS LOURDE, A AJOUTER DU CHLORHYDRATE D'HYDROXYLAMINE A LA SOLUTION DE LADITE 2-CYCLOHEXENE-1-ONE, A AGITER LE MELANGE A REFLUX, A ALCALINISER LE MELANGE ET A L'EVAPORER A SICCITE PUIS A ISOLER DU RESIDU LE PRODUIT RECHERCHE. L'OXIME EST UN INTERMEDIAIRE DE PREPARATION DE LA 3-(4-PYRIDINYL)ANILINE QUI EST ELLE-MEME UN INTERMEDIAIRE DE PREPARATION DE LA ROSOXACINE, AGENT ANTIBACTERIEN.THE INVENTION RELATES TO AN IMPROVED PROCESS FOR THE PREPARATION OF 3- (4-PYRIDINYL) -2-CYCLOHEXENE-1-ONE OXIME FROM 5-OXO-2- (4-PYRIDINYL) CARBONYL ETHYL HEXANOATE IN A SERIES OF REACTIONS IN A SINGLE CONTAINER, WHICH FIRST CONSISTS OF HEATING 5-OXO-2- (4-PYRIDINYL) -ETHYL CARBONYLHEXANOATE WITH AN EXCESS SULFURIC ACID, TO NEUTRALIZE THE EXCESS ACID, TO EXTRACT THE 3- (4-PYRIDINYL) -2-CYCLOHEXENE-1-ONE RESULTING WITH ISOPROPYLIC ALCOHOL, TO REMOVE THE HEAVIER AQUEOUS LAYER, TO ADD HYDROXYLAMINE CHLORHYDRATE TO THE 2-CYCL SOLUTION 1-ONE, AGITATE THE REFLUX MIXTURE, ALKALINIZE THE MIXTURE AND EVAPORATE TO DRY, THEN TO ISOLATE THE RESEARCH PRODUCT FROM THE RESIDUE. OXIME IS AN INTERMEDIATE FOR THE PREPARATION OF 3- (4-PYRIDINYL) ANILINE WHICH IS ITSELF AN INTERMEDIATE FOR THE PREPARATION OF ROSOXACIN, ANTIBACTERIAL AGENT.

Description

Cette invention concerne un procédé amélioré de préparation de la 3-(4-This invention relates to an improved process for preparing 3- (4-

pyridinyl)-2-cyclohexène-1-oxime, un intermédiaire de préparation de la rosoxacine, à partir du -oxo-2-[(4-pyridinyl)carbonyl]hexanoate d'éthyle. Le brevet des E.U.A. N 4.111.946 décrit deux  pyridinyl) -2-cyclohexene-1-oxime, an intermediate for the preparation of rosoxacin, from ethyl -oxo-2 - [(4-pyridinyl) carbonyl] hexanoate. The U.S. Patent N 4,111,946 describes two

séquences de transformation du 5-oxo-2-[(4-pyridinyl)carbonyl]-  5-oxo-2 transformation sequences - [(4-pyridinyl) carbonyl] -

hexanoate d'éthyle en 3-(4-pyridinyl)-2-cyclohexèn-1-one 1) chauffage du 5-oxo-2-[t(4-pyridinyl)-carbonyl]hexanoate d'éthyle dans des conditions acides aqueuses, ce qui hydrolyse ethyl 3- (4-pyridinyl) -2-cyclohexen-1-one hexanoate 1) heating of ethyl 5-oxo-2- [t (4-pyridinyl) -carbonyl] hexanoate under aqueous acid conditions, which hydrolyzes

et décarboxyle le produit en donnant la 1-(4-pyridinyl)- and decarboxylates the product giving 1- (4-pyridinyl) -

hexane-1,5-dione, puis réaction de ladite hexane-1,5-dione hexane-1,5-dione, then reaction of said hexane-1,5-dione

avec un agent de condensation basique pour former la 3-(4- with a basic condensing agent to form 3- (4-

pyridinyl)-2-cyclohexène-1-one; et 2) réaction du 5-oxo-2- pyridinyl) -2-cyclohexene-1-one; and 2) reaction of 5-oxo-2-

[(4-pyridinyl)-carbonyl)]hexanoate d'éthyle avec un agent de [(4-pyridinyl) -carbonyl)] ethyl hexanoate with an agent

condensation basique pour former le 3-(4-pyridinyl)-2-cyclo- basic condensation to form 3- (4-pyridinyl) -2-cyclo-

hexène-l-one-4-carboxylate d'éthyle puis chauffage dudit 4-carboxylate dans des conditions acides aqueuses pour  ethyl hexene-one-4-carboxylate followed by heating of said 4-carboxylate under aqueous acid conditions to

l'hydrolyser et le décarboxyler en vue de former la 3-(4-  hydrolyze and decarboxylate to form 3- (4-

pyridinyl)-2-cyclohexèn-1-one. Puis on fait réagir la 3-(4- pyridinyl) -2-cyclohexen-1-one. Then we react the 3- (4-

pyridinyl)-2-cyclohexène-1-one avec l'hydroxylamine pour la transformer en son oxime, intermédiaire de préparation de la 3-(4-pyridinyl)aniline qui est elle-mêmeun agent intermédiaire de préparation de la rosoxacine, un agent bactérien qui est pyridinyl) -2-cyclohexene-1-one with hydroxylamine to transform it into its oxime, intermediate for the preparation of 3- (4-pyridinyl) aniline which is itself an intermediate agent for the preparation of rosoxacin, a bacterial agent who is

l'acide 1-éthyl-1,4-dihydro-4-oxo-7-(4-pyridinyl)-3-quinoléine-  1-ethyl-1,4-dihydro-4-oxo-7- (4-pyridinyl) -3-quinoline- acid

carboxylique.carboxylic.

L'invention concerne une -amélioration du procédé de transformation du 5oxo-2-[(4-pyridinyl)carbonyl]hexanoate d'éthyle en 3-(4-pyridinyl)-2cyclohexèn-1-one et ensuite de transformation de la cyclohexàne-l-one en son oxime, procédé qui consiste à utiliser une série de réactions dans un seul récipient qui consiste: 1) à chauffer du 5-oxo-2-[(42 pyridinyl) carbonyl]hexanoate d'éthyle avec un excès d'acide sulfurique aqueux, à neutraliser l'excès d'acide, à extraire la 3-(4-pyridinyl)-2-cyclohexène1-one résultante avec de l'alcool isopropylique, à égoutter la couche aqueuse plus lourde, à ajouter du chlorhydrate d'hydroxylamine à la  The invention relates to an improvement of the process for transforming ethyl 5oxo-2 - [(4-pyridinyl) carbonyl] hexanoate into 3- (4-pyridinyl) -2cyclohexen-1-one and then for transforming cyclohexain- l-one to its oxime, process which consists in using a series of reactions in a single container which consists: 1) in heating ethyl 5-oxo-2 - [(42 pyridinyl) carbonyl] hexanoate with an excess of aqueous sulfuric acid, to neutralize excess acid, to extract the resulting 3- (4-pyridinyl) -2-cyclohexene1-one with isopropyl alcohol, to drain the heavier aqueous layer, to add hydrochloride d hydroxylamine

solution d'alcool isopropylique de 3-(4-pyridinyl)-2- 3- (4-pyridinyl) -2- isopropyl alcohol solution

cyclohexèn-l-one, à agiter le mélange à reflux, à alcaliniser le mélange et à l'évaporer à siccité, et à isoler du résidu  cyclohexen-1-one, stirring the mixture at reflux, basifying the mixture and evaporating to dryness, and isolating from the residue

l'oxime de la 3-(4-pyridinyl)-2-cyclohexèn-1-one. 3- (4-pyridinyl) -2-cyclohexen-1-one oxime.

L'invention concerne une amélioration du procédé de préparation de la 3(4-pyridinyl)-2-cyclohexène-1-oxime par chauffage du 5-oxo-2-[(4pyridinyl)carbonyi]hexanoate d'éthyle dans des conditions acides aqueuses pour produire la 1-(4-pyridinyl)-hexane-1,5-dione, par chauffage de ladite hexane-1,5-dione avec un agent de condensation basique pour former ladite 3-(4-pyridinyl)-2-cyclohexène-1-one et la transformation de ladite cyclohexèn-l-one en son oxime, l'amélioration consistant en une série de réactions dans un  The invention relates to an improvement of the process for the preparation of 3 (4-pyridinyl) -2-cyclohexene-1-oxime by heating ethyl 5-oxo-2 - [(4pyridinyl) carbonyi] hexanoate under aqueous acid conditions to produce 1- (4-pyridinyl) -hexane-1,5-dione, by heating said hexane-1,5-dione with a basic condensing agent to form said 3- (4-pyridinyl) -2-cyclohexene -1-one and the transformation of said cyclohexen-l-one into its oxime, the improvement consisting of a series of reactions in a

seul récipient consistant d'abord à chauffer le 5-oxo-2-  only container consisting first of all in heating the 5-oxo-2-

[(4-pyridinyl)carbonyl]hexanoate d'éthyle avec un excès d'acide sulfurique aqueux, à neutraliser l'excès d'acide, à agiter soigneusement le mélange résultant avec de l'alcool  [(4-pyridinyl) carbonyl] ethyl hexanoate with an excess of aqueous sulfuric acid, to neutralize the excess acid, to carefully stir the resulting mixture with alcohol

isopropylique pour extraire la 3-(4-pyridinyl)-2-cyclohexèn- isopropyl to extract 3- (4-pyridinyl) -2-cyclohexèn-

1-one, à égoutter la couche aqueuse chaude (40-50 C) plus lourde, à ajouter du chlorhydrate d'hydroxylamine à la solution de 3-(4-pyridinyl)2-cyclohexèn-1-one dans l'alcool isopropylique, à agiter le mélange à reflux, à alcaliniser le mélange et à l'évaporer à siccité, et à isoler du résidu l'oxime de la 3-(4-pyridinyl)-2-cyclohexèn-1-one. Dans un mode de réalisation préféré, on utilise trois équivalents  1-one, to drain the heavier hot (40-50 C) aqueous layer, to add hydroxylamine hydrochloride to the solution of 3- (4-pyridinyl) 2-cyclohexen-1-one in isopropyl alcohol, stirring the mixture at reflux, basifying the mixture and evaporating to dryness, and isolating the 3- (4-pyridinyl) -2-cyclohexen-1-one oxime from the residue. In a preferred embodiment, three equivalents are used

molaires d'acide sulfurique par mole de 5-oxo-2-[(4-  molars of sulfuric acid per mole of 5-oxo-2 - [(4-

pyridinyl)carbonyl]hexanoate d'éthyle, on neutralise l'excès d'acide sulfurique par une solution aqueuse d'hydroxyde de sodium et on alcalinise le mélange réactionnel, après formation de l'oxime, à l'aide d'hydroxyde d'ammonium concentré. Bien que l'on préfère utiliser trois équivalents  ethyl pyridinyl) carbonyl] hexanoate, the excess sulfuric acid is neutralized with an aqueous solution of sodium hydroxide and the reaction mixture is made alkaline, after formation of the oxime, using hydroxide concentrated ammonium. Although we prefer to use three equivalents

molaires d'acide sulfurique par mole de 5-oxo-2-[(4-pyridinyl)- molars of sulfuric acid per mole of 5-oxo-2 - [(4-pyridinyl) -

carbonyl]hexanoate d'éthyle, on peut en utiliser de deux à quatre équivalents molaires; cependant, on obtient des rendements inférieurs en utilisant moins de trois équivalents molaires et l'utilisation de plus de trois équivalents molaires n'est pas nécessaire. L'alcalinisation par l'hydroxyde d'ammonium après formation de l'oxime amène de préférence le pH entre 7 et 8. L'oxime est commodément et de préférence isoléeà partir de sels minéraux, le plus souvent le chlorure d'ammonium, en utilisant un alcanol aqueux, de préférence en chauffant le résidu avec de l'eau ethyl carbonyl] hexanoate, two to four molar equivalents can be used; however, lower yields are obtained by using less than three molar equivalents and the use of more than three molar equivalents is not necessary. Alkalinization with ammonium hydroxide after formation of the oxime preferably brings the pH between 7 and 8. The oxime is conveniently and preferably isolated from mineral salts, most often ammonium chloride, in particular using an aqueous alkanol, preferably by heating the residue with water

à environ 60 à 80 C puis en ajoutant de l'éthanol.  at around 60 to 80 C and then adding ethanol.

Le procédé amélioré de l'invention présente un certain nombre d'avantages par rapport à celui du brevet des E.U.A. N 4.111.946, à savoir: 1) il fournit une réaction simplifiée en un seul récipient plutôt que plusieurs étapes séparées; 2) il évite les étapes séparées de chauffage du 5-oxo-2[(4-pyridinyl)carbonyl]hexanoate d'éthyle dans des  The improved method of the invention has a number of advantages over that of the U.S. patent. N 4,111,946, namely: 1) it provides a simplified reaction in a single container rather than several separate stages; 2) it avoids the separate steps of heating ethyl 5-oxo-2 [(4-pyridinyl) carbonyl] hexanoate in

conditions acides aqueuses pour produire la 1-(4-pyridinyl)-  aqueous acid conditions to produce 1- (4-pyridinyl) -

hexan-l,5-dione et le chauffage de la 1,5-dione avec un agent hexan-l, 5-dione and heating 1,5-dione with an agent

de condensation basique pour obtenir la 3-(4-pyridinyl)-2- of basic condensation to obtain 3- (4-pyridinyl) -2-

cyclohexène-l-one; 3) il utilise considérablement moins (un tiers) d'acide sulfurique, par exemple seulement trois  cyclohexene-1-one; 3) it uses considerably less (a third) of sulfuric acid, for example only three

équivalents molaires au lieu des neuf par mole de 5-oxo-2-  molar equivalents instead of nine per mole of 5-oxo-2-

[(4-pyridinyl)carbonyl]hexanoate d'éthyle utilisés dans ce brevet, ce qui nécessite ensuite nettement moins de solution d'hydroxyde de sodium et qui réduit le volume du mélange réactionnel; 4) il utilise l'alcool isopropylique comme agent d'extraction de la 3-(4-pyridinyl)-2-cyclohexèn1-one, en remplaçant ainsi le chloroforme et en permettant la vidange commode de la couche aqueuse lourde non désirée; 5) il transforme directement la 2-cyclohexèn-1-one dans l'extrait d'alcool isopropylique en son oxime; et 6) il évite les étapes de purification de préparation et de recristallisation du méthanesulfonate de l'oxime. L'oxime préparée par le procédé amélioré de l'invention peut êtreutilisée directement, Ethyl [(4-pyridinyl) carbonyl] hexanoate used in this patent, which then requires significantly less sodium hydroxide solution and which reduces the volume of the reaction mixture; 4) it uses isopropyl alcohol as an extracting agent for 3- (4-pyridinyl) -2-cyclohexen1-one, thereby replacing the chloroform and allowing the convenient drainage of the unwanted heavy aqueous layer; 5) it directly transforms 2-cyclohexen-1-one in the isopropyl alcohol extract into its oxime; and 6) it avoids the purification steps of preparation and recrystallization of the methanesulfonate from the oxime. The oxime prepared by the improved process of the invention can be used directly,

sans autre purification, pour sa transformation en N-acétyl- without further purification, for its transformation into N-acetyl-

3-(4-pyridinyl)aniline par l'intermédiaire du dérivé O- 3- (4-pyridinyl) aniline via the O- derivative

acétylé. L'exemple suivant illustrera l'invention sans acetylated. The following example will illustrate the invention without

toutefois la limiter.however limit it.

A une solution refroidie et agitée de 250 ml (4,49 moles) d'acide sulfurique concentré dans 800 ml d'eau,  To a cooled and stirred solution of 250 ml (4.49 moles) of concentrated sulfuric acid in 800 ml of water,

on ajoute 390 g (1,48 mole) de S-oxo-2-[(4-pyridinyl)-  390 g (1.48 mole) of S-oxo-2 - [(4-pyridinyl) - are added

carbonyl]hexanoate d'éthyle à une vitesse telle que l'on maintient la température en-dessous de 20 C. Le récipient de réaction est relié par l'intermédiaire d'un réfrigérant à refroidissement d'eau dirigé vers le bas et d'un récepteur à un appareil de mesure du volume de gaz destiné à mesurer le dégagement de gaz carbonique. La solution légèrement trouble est agitée à la température ambiante pendant une nuit. Après 16 heures d'agitation, 15 % de la quantité théorique de gaz carbonique se sont dégagés. [Dans un autre essai' 41 % de gaz carbonique se sont dégagés quand le mélange réactionnel a été agité pendant 65 heures]. Puis on chauffe progressivement la solution brun clair maintenant limpide sur un bain dé vapeur jusqu'à 920C en trois heures, chauffage qui s'accompagne d'un dégagement gazeux de plus en plus vigoureux Période totale de Température interne chauffage (h) OC % de CO2 dégagé ethyl carbonyl] hexanoate at such a rate that the temperature is kept below 20 C. The reaction vessel is connected via a water-cooled refrigerant directed downwards and a receiver to a device for measuring the volume of gas intended to measure the evolution of carbon dioxide. The slightly cloudy solution is stirred at room temperature overnight. After 16 hours of stirring, 15% of the theoretical amount of carbon dioxide was released. [In another test '41% of carbon dioxide was released when the reaction mixture was stirred for 65 hours]. Then the light brown solution, now limpid, is gradually heated on a steam bath up to 920C in three hours, heating which is accompanied by an increasingly vigorous evolution of gas Total period of internal temperature heating (h) OC% of CO2 released

0 25 150 25 15

0,5 30 160.5 30 16

1 49 201 49 20

1,5 59 271.5 59 27

2 68 392 68 39

2,5 80 602.5 80 60

3 92 993 92 99

Pendant les 40 minutes suivantes à 920C, le dégagement de gaz s'arrête pratiquement. On refroidit le mélange réactionnel foncé à 40'C et on l'alcalinise avec environ 800 ml d'hydroxyde de sodium aqueux à 35 %, en refroidissant quand besoin est pour maintenir la température près de 400C. On prélève l'huile qui se sépare avec 660 ml d'alcool isopropylique et on sépare la couche aqueuse plus lourde pendant qu'elle est encore chaude (40 à 50'C) et on la rejette. La solution dans l'alcool isopropylique contenant la 3-(4-pyridinyl)-2-cyclohexèn-1-one est utilisée dans l'étape suivante de formation d'oxime. A l'alcool isopropylique contenant la 2cyclohexèn-1-one, on ajoute 120 g (1,72 mole) de chlorhydrate d'hydroxylamine et on agite le mélange à reflux pendant deux heures. On alcalinise la solution encore chaude avec environ 200 ml d'hydroxyde d'ammonium concentré. On évapore le mélange réactionnel à  During the next 40 minutes at 920C, the gas evolution practically stops. The dark reaction mixture is cooled to 40 ° C and made alkaline with about 800 ml of 35% aqueous sodium hydroxide, cooling when necessary to keep the temperature near 400C. The oil which separates is removed with 660 ml of isopropyl alcohol and the heavier aqueous layer is separated while it is still hot (40 to 50 ° C.) and it is discarded. The solution in isopropyl alcohol containing 3- (4-pyridinyl) -2-cyclohexen-1-one is used in the next stage of oxime formation. To the isopropyl alcohol containing 2cyclohexen-1-one, 120 g (1.72 mole) of hydroxylamine hydrochloride are added and the mixture is stirred at reflux for two hours. The still hot solution is made alkaline with about 200 ml of concentrated ammonium hydroxide. The reaction mixture is evaporated at

siccité sous vide et l'on obtient un mélange d'oxime de 3-(4-  dry in vacuo and an oxime mixture of 3- (4-

pyridinyl)-2-cyclohexèn-1-one et de sels minéraux, essentiellement du chlorure d'ammonium. On agite le résidu et on le chauffe dans 680 ml d'eau à 70 C et l'on ajoute 340 ml d'éthanol absolu. On laisse le mélange refroidir lentement jusqu'à la température ambiante en l'agitant et on le refroidit dans un bain de glace avant de filtrer le solide beige clair. On lave soigneusement le produit avec de l'eau et on le sèche à 60 C sous vide et l'on obtient 236 g (84,8%)  pyridinyl) -2-cyclohexen-1-one and mineral salts, mainly ammonium chloride. The residue is stirred and heated in 680 ml of water at 70 ° C. and 340 ml of absolute ethanol are added. The mixture is allowed to cool slowly to room temperature with stirring and cooled in an ice bath before filtering the light beige solid. The product is washed carefully with water and dried at 60 ° C. under vacuum and 236 g (84.8%) are obtained

d'oxime de 3-(4-pyridinyl)-2-cyclohexèn-1-one, p.f. 172-181 C.  3- (4-pyridinyl) -2-cyclohexen-1-one oxime, m.p. 172-181 C.

Son spectre RMN n'indique pas la présence d'impuretés.  Its NMR spectrum does not indicate the presence of impurities.

Claims (4)

REVENDICATIONS 1. Procédé de préparation de l'oxime de la 3-(4- 1. Process for preparing the oxime of 3- (4- pyridinyl)-2-cyclohexèn-1-one par chauffage du 5-oxo-2-[(4- pyridinyl) -2-cyclohexen-1-one by heating 5-oxo-2 - [(4- pyridinyl)carbonyl]hexanoate d'éthyle dans des conditions acides aqueuses pour former la 1-(4-pyridinyl)-hexane-1,5- dione, chauffage de ladite hexane-1,5-dione avec un agent de  ethyl pyridinyl) carbonyl] hexanoate under aqueous acid conditions to form 1- (4-pyridinyl) -hexane-1,5-dione, heating said hexane-1,5-dione with an agent condensation basique pour former la 3-(4-pyridinyl)-2-cyclo-  basic condensation to form 3- (4-pyridinyl) -2-cyclo- hexèn-1-one et transformation de ladite cyclohexèn-1-one en son oxime, caractérisé en ce qu'il comprend une série de réactions dans un seul récipient consistant à chauffer d'abord du 5-oxo-2-[(4-pyridinyl)carbonyl] hexanoate d'éthyle avec un excès d'acide sulfurique aqueux, à neutraliser l'excès d'acide, à agiter soigneusement le mélange chaud résultant avec de  hexen-1-one and transformation of said cyclohexen-1-one into its oxime, characterized in that it comprises a series of reactions in a single container consisting in first heating 5-oxo-2 - [(4- pyridinyl) carbonyl] ethyl hexanoate with an excess of aqueous sulfuric acid, to neutralize the excess acid, to carefully stir the resulting hot mixture with l'alcool isopropylique pour extraire la 3-(4-pyridinyl)-2- isopropyl alcohol to extract 3- (4-pyridinyl) -2- cyclohexèn-l-one, à enlever la couche aqueuse chaude plus lourde, à ajouter du chlorhydrate d'hydroxylamine à la solution de 3-(4-pyridinyl)2-cyclohexèn-1-one dans l'alcool isopropylique, à agiter le mélange à reflux, à alcaliniser le mélange et à l'évaporer à siccité, et à isoler du résidu  cyclohexen-1-one, to remove the heavier hot aqueous layer, to add hydroxylamine hydrochloride to the solution of 3- (4-pyridinyl) 2-cyclohexen-1-one in isopropyl alcohol, to stir the mixture at reflux, alkalinize the mixture and evaporate to dryness, and isolate from the residue l'oxime de la 3-(4-pyridinyl)-2-cyclohexèn-1-one.  3- (4-pyridinyl) -2-cyclohexen-1-one oxime. 2. Procédé selon la revendication 1, caractérisé en ce qu'on utilise trois équivalents molaires d'acide sulfurique 2. Method according to claim 1, characterized in that three molar equivalents of sulfuric acid are used par mole de 5-oxo-2-[(4-pyridinyl)carbonyl]hexanoate d'éthyle. per mole of ethyl 5-oxo-2 - [(4-pyridinyl) carbonyl] hexanoate. 3. Procédé selon l'une ou l'autre des revendications 3. Method according to either of the claims 1 et 2, caractérisé en ce qu'on neutralise l'excès d'acide  1 and 2, characterized in that the excess acid is neutralized sulfurique avec une solution aqueuse d'hydroxyde de sodium. sulfuric with an aqueous solution of sodium hydroxide. 4. Procédé selon l'une quelconque des  4. Method according to any one of revendications 1, 2 et 3, caractérisé en ce qu'on alcalinise  Claims 1, 2 and 3, characterized in that it is made alkaline le mélange réactionnel, après formation de l'oxime, avec de l'hydroxyde d'ammonium concentré jusqu'à un pH compris entre  the reaction mixture, after formation of the oxime, with concentrated ammonium hydroxide up to a pH of between 7 et 8.7 and 8.
FR8021518A 1979-12-19 1980-10-08 PROCESS FOR THE PREPARATION OF OXIME OF 3- (4-PYRIDINYL) -2-CYCLOHEXENE-1-ONE Pending FR2471977A1 (en)

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